Femtosecond electron microscopy produces real-space images of matter in a series of ultrafast snapshots. Pulses of electrons self-disperse under space-charge broadening, so without compression, the ideal operation mode is a single electron per pulse. Here, we demonstrate femtosecond single-electron point projection microscopy (fs-ePPM) in a laser-pump fs-e-probe configuration. The electrons have an energy of only 150 eV and take tens of picoseconds to propagate to the object under study. Nonetheless, we achieve a temporal resolution with a standard deviation of 114 fs (equivalent to a full-width at half-maximum of 269 ± 40 fs) combined with a spatial resolution of 100 nm, applied to a localized region of charge at the apex of a nanoscale metal tip induced by 30 fs 800 nm laser pulses at 50 kHz. These observations demonstrate real-space imaging of reversible processes, such as tracking charge distributions, is feasible whilst maintaining femtosecond resolution. Our findings could find application as a characterization method, which, depending on geometry, could resolve tens of femtoseconds and tens of nanometres. Dynamically imaging electric and magnetic fields and charge distributions on sub-micron length scales opens new avenues of ultrafast dynamics. Furthermore, through the use of active compression, such pulses are an ideal seed for few-femtosecond to attosecond imaging applications which will access sub-optical cycle processes in nanoplasmonics.

A novel application of velocity-map imaging (VMI) is demonstrated, whereby the momentum distribution of photoelectrons ejected from a tungsten nanoscale metal tip (<50 nm radius) is recorded following illumination with an ultrafast laser pulse. The electrostatic conditions in the VMI instrument are optimized through finite element modelling, taking into account a physically realistic geometry including all conductive elements in the vicinity of the electron trajectories. The instrument is calibrated by observing above threshold ionization in krypton gas, and simultaneous electron emission from this gas and a tungsten nanotip is presented, illustrating that the velocity mapping condition is maintained. Realizing photoelectron VMI for femtosecond laser illuminated nanoscale objects will have a significant impact on the emerging field of ultrafast nanoplasmonics and will influence the development of such devices as a source of coherent pulses of electrons with applications in time-resolved microscopy, holography and diffractive imaging.

Femtosecond vacuum ultraviolet pulses from a monochromated high harmonic generation source excite vibrational wavepackets in the B 1 g S + state of D 2 . The wavepacket motion is measured through strong field ionization into bound and dissociative ion states yielding D 2 + and D + products. The time dependence of the D 2 + and D + ion signals provides a sensitive fingerprint of the quantum nuclear wavepacket, due to the different ionization rates for the two channels. The experiments are modelled with excitation and ionization processes included explicitly, with the results of the model showing a very good agreement with the experimental observations. The experiment demonstrates the level of detail attainable when studying ultrafast quantum nuclear dynamics using high harmonic sources.

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